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研究生: 陳俊安
Chen, Jiun-an
論文名稱: 分子模版應用於香菸主流煙中多環芳香烴分析方法之研發
Method Development of Molecular Imprinting Polymers for the Analysis of PAHs in the Mainstream Smoke from Cigarettes.
指導教授: 林達昌
Lin, Ta-cheng
學位類別: 碩士
Master
系所名稱: 工學院 - 環境工程學系
Department of Environmental Engineering
論文出版年: 2009
畢業學年度: 97
語文別: 中文
論文頁數: 103
中文關鍵詞: 香菸主流煙多環芳香族化合物PAHsBenzo[a]pyrene (BaP)7-methylbenzo[a]pyrene(7-MeBP)分子模版
外文關鍵詞: Benzo[a]pyrene, PAHs, mainstream smoke, molecular imprinted polymers, 7-methylbenzo[a]pyrene
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  • 本研究是利用分子模版技術,萃取環境樣品中多環芳香族化合物(PAHs),並且利用分子模版之特性,更有效的萃取出PAHs中之有毒物質Benzo[a]pyrene (BaP),研究中透過各種材料測試,以及採集市售香煙主流煙進行分析,所採集之樣品由氣相層析質譜儀(GC/MS)進行分析。
    分子模版主要是經由官能基單體與交聯劑之間的作用,對於目標吸附物質形成特殊孔洞,以達到選擇性的萃取之目的。本研究室自行研發之分子模版,以結構相似之7-methylbenzo[a]pyrene(7-MeBP)作為目標分子製備模版,透過分子模版的高選擇性,有效的吸附目標汙染物,且與傳統萃取技術比較,不僅可以減少時間、人力,使用溶劑也較少。
    本實驗依照不同官能基單體與交聯劑,配置三種不同配比之分子模版,在目標分子的移除之後,分為控制組及對照組,進行各種材料測試,如:吸附量測試、選擇性測試、回收率測試、環境樣品測試、掃描式電子顯微鏡(SEM)等,實驗結果顯示,MIP-1為效果最佳之分子模版,其吸附容量為20.78 ± 1.7 (μg/g),針對BaP的選擇性與回收率皆為90 %以上,而在環境樣品測試部份,分為Mild Seven sky blue(七星淡菸)及Marlboro light(萬寶路淡菸)兩種香菸之主流煙測試,分子模版所吸附之BaP量,為濾紙採樣吸附之80 %。由各項結果顯示,分子模版可以有效的吸附16 種PAHs中之BaP分子,且可降低儀器分析背景值之干擾,提高訊號解析度。此外與傳統萃取方式相較,分子模版運用於前處理的方式,可以有效地降低在前處理時的人力、時間與有機溶劑的消耗,改良傳統前處理之缺點。

    Polycyclic aromatic hydrocarbons (PAHs) and their derivatives are common trace pollutants produced during incomplete combustion of organic substances such as tobacco. After sampling cigarette smoke, PAH collators must undergo pretreatment processes such as extraction, cleanup and concentration before instrument analysis. This study combines molecular imprinted polymers (MIPs) and solid-phase extraction (SPE) to create a novel sample pretreatment technique.
    Experimental results demonstrate that MIPs have good selectivity for Benz[a]Pyrene (BaP) from a mixture of 16 PAH solvents. The MIPs were applied to a sample taken from mainstream smoke from a cigarette. Based on functional monomers and cross-linkers, this study investigated three groups of MIPs. After the template was removed, various tests, including capacity, selectivity, recovery, scanning electron microscope (SEM) observations and real environmental sample tests, were conducted. Experimental results show that MIP-1 is the best MIP with a capacity of 20.78 ± 1.7 (μg/g), BaP selectivity and recovery exceeding 93%. In environmental sample tests, i.e., main stream smoke from S and M brand cigarettes, 80% of BAP was absorbed by MIP compared with that absorbed by filters. All experimental results suggest that MIPs effectively adsorbed BaP among 16 different PAHs, reduced background interference and increased signal resolution compared with traditional extraction techniques.
    Additionally, using MIPs for sample pretreatment is less laborious than traditional sample pretreatments. It saves time and reduces organic solvent reduces consumption. Using molecular imprinted polymers solid extraction (MISPE) may separate target analytes from a complex sample more effectively than traditional Soxhlet extraction. Future toxicity tests should contribute to the understanding of toxic compounds emitted from specific pollution sources.

    總目錄 摘要 I 誌謝 V 總目錄 VII 表目錄 X 第一章 前言 1 1-1 研究動機 1 1-2 研究目的 2 第二章 文獻回顧 3 2-1 微量分析之概念與應用 3 2-1-1 微量分析技術 3 2-1-2 微量分析與樣品前處理 4 2-2 固相萃取之概念與應用 7 2-2-1 固相萃取原理與流程 7 2-2-2 固相萃取與微量物質分析 8 2-3 分子模版之概念與應用 9 2-3-1 分子模版歷史沿革 9 2-3-2 分子模版概念 10 2-3-3 分子模版與固相萃取的結合 10 2-3-4 分子模版與傳統萃取的比較 11 2-4 市售香菸之危害性 13 2-4-1 香菸燃燒特性 13 2-4-2 香菸燃燒的有害物質 15 2-5 PAHs之特性及危害性 19 2-5-1 PAHs的性質與來源 19 2-5-2 PAHs的形成與致癌機制 20 2-5-3 16種PAHs的結構與毒性 21 2-5-4 BaP與7-MeBP的特性及危害性 28 第三章 實驗方法與步驟 29 3-1 實驗藥品與器材 29 3-1-1 目標分子 29 3-1-2 起始劑 29 3-1-3 官能基單體 29 3-1-4 交聯劑 30 3-2 分子模版之製備 31 3-2-1 製備配比 31 3-2-2 製備流程 32 3-2-3 熱聚合與脫模程序 34 3-3 PAHs之分析方法 35 3-4 實驗設計與規劃 36 3-5 吸附量測試 37 3-5 吸附量測試 38 3-7 回收率測試 39 3-8 貫穿量測試 39 3-9 環境樣品測試 40 3-9-1 採樣設計與規劃 40 3-9-2 採樣地點 41 3-9-3 濾紙採樣與分析 41 3-9-4 分子模版採樣與分析 45 3-10 重複使用性測試 48 3-11 掃描式電子顯微鏡(SEM)觀察 49 第四章 數據分析之品質保證與控制 50 4-1 PAHs空白試驗 50 4-1-1 溶劑空白試驗 50 4-1-2 程序空白試驗 50 4-2 標準品檢量線之建立 52 4-2-1 建立檢量線 52 4-2-2 線性關係之確認 52 4-2-3 濃度可適用之範圍 52 4-2-4 檢量線的確認及使用 52 第五章 結果與討論 57 5-1 吸附容量測試結果 57 5-2 選擇性測試結果 58 5-3 回收率測試結果 61 5-4 貫穿量測試結果 63 5-5 市售香煙採樣分析結果 64 5-6 重複使用性測試結果 72 5-7 SEM觀察結果 75 第六章 結論與建議 79 參考文獻 81 Appendix A 16種PAHs之檢量線(GC/MS) 87 自述 103

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